Gaussian curvature engineering of self-pressurizing mesoporous nanoreactors boosts dynamic equilibrium of molecule adsorption-desorption.

Li, Jinying; Guo, Shenghong; Guo, Peiting; Zhu, Youliang; Wang, Aixia; Zhang, Jiaming; Kang, Tianke; Wu, Limin et al. · Nat Commun · 2025

basic_science · Level V

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Abstract

Modulating the molecule adsorption-desorption behaviors of solid catalysts is important for fulfilling complicated catalytic purposes. Herein, we quantitatively reveal the dynamic balancing of molecule adsorption/desorption by curvature modulation on a series of self-pressurizing mesoporous nanoreactors with controlled concave-convex Gaussian curvatures via a programmable nanodroplet buckling strategy. The encapsulation of Fe<sub>3</sub>O<sub>4</sub> nanoparticles in the cavity produces a large temperature difference between the nanoreactor surface (193.8 °C) and the reaction medium (73.7 °C) under photoexcitation, forming thermally confined self-pressurizing nanoreactors. Together with the external pressure exerted by the liquid-surface-tension on the concave-convex surfaces, the self-pressurizing drives the dynamic regulation of molecule adsorption-desorption on the Gaussian surface. Based on this, the nanoreactor with catalytic metallic Ru on the outer shells achieves the high-selective cascade oxidation of biomass-derived 5-hydroxymethylfurfural to high-value-added 5-formyl-2-furancarboxylic acid (97.9% selectivity), showing a reaction efficiency that is an order of magnitude higher than that of conventional heating.